To overcome the ever-growing organic pollutions in the water system, abundant efforts have been dedicated to fabricating efficient Fenton-like carbon catalysts. However, the rational design of carbon catalysts with high intrinsic activity remains a long-term goal. Herein, we report a new N-molecule-assisted self-catalytic carbonization process in augmenting the intrinsic Fenton-like activity of metal–organic-framework-derived carbon hybrids. During carbonization, the N-molecules provide alkane/ammonia gases and the formed iron nanocrystals act as the in situ catalysts, which result in the elaborated formation of carbon nanotubes (in situ chemical vapor deposition from alkane/iron catalysts) and micro-/meso-porous structures (ammonia gas etching). The obtained catalysts exhibited with abundant Fe/Fe–N_x/pyridinic-N active species, micro-/meso-porous structures, and conductive carbon nanotubes. Consequently, the catalysts exhibit high efficiency toward the degradation of different organic pollutions, such as bisphenol A, methylene blue, and tetracycline. This study not only creates a new pathway for achieving highly active Fenton-like carbon catalysts but also takes a step toward the customized production of advanced carbon hybrids for diverse energy and environmental applications.

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为了克服水系统中日益增长的有机污染，已致力于制造高效的类似于Fenton的碳催化剂。然而，合理设计具有高固有活性的碳催化剂仍然是一个长期目标。在这里，我们报道了一种新的由N分子辅助的自催化碳化过程，可以增强金属-有机骨架衍生的碳杂种的固有Fenton样活性。碳化过程中，氮分子提供烷烃/氨气，形成的铁纳米晶体充当原位催化剂，从而导致碳纳米管（烷烃/铁催化剂的原位化学气相沉积）和微孔/中孔结构（氨）的精细形成气体蚀刻）。所获得的催化剂具有丰富的Fe / Fe–N _x/吡啶-N活性物质，微孔/中孔结构和导电碳纳米管。因此，该催化剂对降解不同的有机污染物如双酚A，亚甲基蓝和四环素具有很高的效率。这项研究不仅为获得高活性的Fenton类碳催化剂创造了一条新途径，而且还朝着定制生产先进的碳杂化体迈出了一步，以用于各种能源和环境应用。

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